Block copolymers are well-known for their ability to form nanostructures through microphase separation. These nanostructures provide useful and novel mechanical properties to materials ranging from rubber tires to biomedical devices. Formation of the core-shell sphere morphology by ABC triblock copolymers is being studied to create a fracture and fatigue resistant hydrogel. While AB diblock polymer morphology has been extensively studied, ABC triblock polymer study has yet to build a comprehensive phase diagram especially in the regions of large volume fractions of the A or C end block. This presentation will highlight the study of this phase region with polystyrene-polyisoprene-poly(ethylene oxide) (PS-PI-PEO) polymers and explore the preparation and mechanical study of hydrogels made with these PS-PI-PEO polymers.